Soot particle (black carbon) morphology is of dual interest, both from a health perspective and due to the influence of soot on the global climate. In this study, the mass-mobility relationships, and thus effective densities, of soot agglomerates from three types of soot emitting sources were determined in situ by combining a differential mobility analyzer (DMA) and an aerosol particle mass analyzer (APM). High-resolution transmission electron microscopy was also used. The soot sources were diesel engines, diffusion flame soot generators, and tapered candles, operated under varying conditions. The soot microstructure was found to be similar for all sources and settings tested, with a distance between the graphene layers of 3.7-3.8 Å. The particle specific surface area was found to vary from 100 to 260 m 2 /g. The particle mass-mobility relationship could be described by a power law function with an average exponent of 2.3 (±0.1) for sources with a volatile mass fraction <10% and primary particle sizes of 11-29 nm. The diesel exhaust from a heavy duty engine at idling had a substantially higher volatile mass fraction and a higher mass-mobility exponent of 2.6. The mass-mobility exponent was essentially independent of the number of primary particles in the range covered (N pp = 10-1000). Despite the similar exponents, the effective density varied substantially from source to source. Two parameters were found to alter the effective density: primary particle size and coating mass fraction. A correlation was found between primary particle size and mass-mobility relationship/effective density and an empirical Address correspondence to Jenny Rissler, Ergonomics and Aerosol Technology, Lund University, P.O. Box 118, SE-221 00, Lund, Sweden. E-mail: jenny.rissler@design.lth.se expression relating these parameters is presented. The effects on the DMA-APM results of doubly charged particles and DMA agglomerate alignment were investigated and quantified. Finally, the dataset was compared to three theoretical approaches describing agglomerate particles' mass-mobility relationship.
Miniaturized detection systems for nanometer-sized airborne particles are in demand, for example in applications for onboard diagnostics downstream particulate filters in modern diesel engines. A soot sensor based on resistivity measurements was developed and characterized. This involved generation of soot particles using a quenched co-flow diffusion flame; depositing the particles onto a sensor substrate using thermophoresis and particle detection using a finger electrode structure, patterned on thermally oxidized silicon substrate. The generated soot particles were characterized using techniques including Scanning Mobility Particle Sizer for mobility size distributions, Differential Mobility Analyzer-Aerosol Particle Mass analyzer for the mass-mobility relationship, and Transmission Electron Microscopy for morphology. The generated particles were similar to particles from diesel engines in concentration, mobility size distribution, and mass fractal dimension. The primary particle size, effective density and organic mass fraction were slightly lower than values reported for diesel engines. The response measured with the sensors was largely dependent on particle mass concentration, but increased with increasing soot aggregate mobility size. Detection down to cumulative mass as small as 20-30 µg has been demonstrated. The detection limit can be improved by using a more sensitive resistance meter, modified deposition cell, larger flow rates of soot aerosol and modifying the sensor surface.
Production of synthesis gas by catalytic reforming of product gas from biomass gasification can lead to catalyst deactivation by the exposure to ash compounds present in the flue gas. The impact of fly ash from biomass gasification on reforming catalysts was studied at the laboratory scale. The investigated catalyst was Pt/Rh based, and it was exposed to generated K2SO4 aerosol particles and to aerosol particles produced from the water-soluble part of biomass fly ash, originating from a commercial biomass combustion plant. The noble metal catalyst was also compared with a commercial Ni-based catalyst, exposed to aerosol particles of the same fashion. To investigate the deactivation by aerosol particles, a flow containing submicrometer-size selected aerosol particles was led through the catalyst bed. The particle size of the poison was measured prior to the catalytic reactor system. Fresh and aerosol particle exposed catalysts were characterized using BET surface area, XRPD (X-ray powder diffraction), and H2 chemisorption. The Pt/Rh catalyst was also investigated for activity in the steam methane reforming reaction. It was found that the method to deposit generated aerosol particles on reforming catalysts could be a useful procedure to investigate the impact of different compounds possibly present in the product gas from the gasifier, acting as potential catalyst poisons. The catalytic deactivation procedure by exposure to aerosol particles is somehow similar to what happens in a real plant, when a catalyst bed is located subsequent to a biomass gasifier or a combustion boiler. Using different environments (oxidizing, reducing, steam present, etc.) in the aerosol generation adds further flexibility to the suggested aerosol deactivation method. It is essential to investigate the deactivating effect at the laboratory scale before a full-scale plant is taken into operation to avoid operational problems.
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